Characterizing and Overcoming Surface Paramagnetism in Magnetoelectric Antiferromagnets

Abstract

We use a combination of density functional theory and Monte Carlo methods to calculate the surface magnetization in magnetoelectric Cr2O3 at finite temperatures. Such antiferromagnets, lacking both inversion and time-reversal symmetries, are required by symmetry to possess an uncompensated magnetization density on particular surface terminations. Here, we first show that the uppermost layer of magnetic moments on the ideal (001) surface remains paramagnetic at the bulk Néel temperature, bringing the theoretical estimate of surface magnetization density in line with experiment. We demonstrate that the lower surface ordering temperature compared to bulk is a generic feature of surface magnetization when the termination reduces the effective Heisenberg coupling. We then propose two methods by which the surface magnetization in Cr2O3 could be stabilized at higher temperatures. Specifically, we show that the effective coupling of surface magnetic ions can be drastically increased either by a different choice of surface Miller plane, or by Fe doping. Our findings provide an improved understanding of surface magnetization properties in AFMs.